Removal performance of norfloxacin from waters by advanced oxidation processes based on different free radicals
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摘要: 抗生素在水中的赋存浓度较低,难以被常规的城市污水处理系统有效去除。考察了紫外光联合氯(UV/氯)、双氧水(UV/H2O2)、过硫酸盐(UV/PS) 3种高级氧化体系对诺氟沙星(NFX)的去除效果。结果表明:UV/氯体系降解NFX相比于其他2种具有显著的高效性,当溶液初始pH为7、氯浓度为30 μmol/L时,NFX在2 min内的去除率可达98.67%,相同氧化剂浓度下,UV/H2O2和UV/PS体系10 min内对NFX的去除率仅为41.41%和65.73%;对于UV/氯体系,NFX的去除率随氯浓度的升高而上升,同时考虑成本,最优氯浓度为30 μmol/L;pH影响3种体系对NFX的去除速率,但效果不同,对于UV/氯体系,强碱性条件有利于NFX的去除,对于UV/H2O2和UV/PS体系,中性及弱碱性更有利于NFX的去除;水体基质Cl-对UV/氯体系去除NFX有抑制作用,但对UV/H2O2和UV/PS体系影响不大;
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关键词:
- 抗生素 /
- 诺氟沙星 /
- UV/氯 /
- 高级氧化技术(AOPs)
Abstract: Because of their low occurrence concentration in water, the antibiotics are difficult to be effectively removed by the conventional municipal sewage treatment system. The removal efficiency of norfloxacin (NFX) by ultraviolet combined chlorine (UV/chlorine), hydrogen peroxide (UV/H2O2) and persulfate (UV/PS) was investigated. The results showed that the degradation of NFX by UV/chlorine was significantly more efficient than the other two systems. When the initial pH of solution was 7 and the concentration of chlorine was 30 μmol/L, the removal rate of NFX in 2 min could reach 98.67%. At the same oxidant concentration, the removal rate of NFX was 41.41% and 65.73% after 10 min by UV/H2O2 and UV/PS, respectively. For UV/chlorine system, the removal rate of NFX increased with the increase of chlorine concentration with the optimal concentration being 30 μmol/L. The pH had different effects on the removal rate of NFX by three systems. For UV/chlorine system, strong alkaline condition was beneficial for the removal of NFX, while neutral and weak alkalinity was more favorable for the removal of NFX for UV/H2O2 and UV/PS. Cl-in water matrix inhibited the removal of NFX by UV/chlorine, but had little effect on UV/H2O2 and UV/PS, while-
Keywords:
- antibiotics /
- norfloxacin /
- UV/chlorine /
- advanced oxidation processes(AOPs)
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[1] 吴曼琳 . 城市水环境中药品和个人护理用品的研究现状和去除[J]. 净水技术, 2018,37(增刊1):230-234. WU M L . Research status and removal of pharmaceuticals and personal care products in urban water environment[J]. Water Purification Technology, 2018,37(Suppl 1):230-234.
[2] 施文杰, 王长友, 杨锐 . 诺氟沙星对盐生杜氏藻、新月菱形藻和小球藻的生态毒性效应[J]. 海洋环境科学, 2019,38(1):1-6. SHI W J, WANG C Y, YANG R . Effects of norfloxacin on Dunaliella salina,Nitzschia closterium F. minutissima and Chlorella vulgaris[J]. Marine Environmental Science, 2019,38(1):1-6.
[3] 郭隽, 张亚雷, 周雪飞 , 等. 城市污水中氟氟喹诺酮类抗生素药物的来源与去除研究进展[J]. 环境污染与防治, 2016,38(2):75-80. GUO J, ZHANG Y L, ZHOU X F , et al. Occurrence and removal of fluoroquinolones in municipal sewage:a review[J]. Environmental Pollution & Control, 2016,38(2):75-80.
[4] 李华瑞, 梁立锐, 程士 , 等. 水中诺氟沙星污染现状及其处理方法研究进展[J]. 山东化工, 2015,44(15):60-62. LI H R, LIANG L R, CHENG S , et al. Research progress in the pollution situation and treatment methods for norfloxacin in water[J]. Shandong Chemical Industry, 2015,44(15):60-62.
[5] 陈凯杰 . 试论饮用水中抗生素去除技术研究进展[J]. 科技经济导刊, 2018,26(8):103-105. [6] 张玮玮, 弓爱君, 邱丽娜 , 等. 废水中抗生素降解和去除方法的研究进展[J]. 中国抗生素杂志, 2013,38(6):401-410. ZHANG W W, GONG A J, QIU L N , et al. Processes of degradation and removal methods of antibiotics from waste water[J]. Chinese Journal of Antibiotics, 2013,38(6):401-410.
[7] 李博 . 莲杆活性炭对诺氟沙星吸附性的研究[D]. 济南:山东大学, 2011. [8] DORIVAL-GARCÍA N, ZAFRA-GOMEZ A, NAVALON A , et al. Removal and degradation characteristics of quinolone antibiotics in laboratory-scale activated sludge reactors under aerobic,nitrifying and anoxic conditions[J]. Journal of Environmental Management, 2013,120:75-83.
doi: 10.1016/j.jenvman.2013.02.007 pmid: 23507246[9] YANG X, FLOWERS R C, WEINBERG H S , et al. Occurrence and removal of pharmaceuticals and personal care products(PPCPs) in an advanced wastewater reclamation plant[J]. Water Research, 2011,45(16):5218-5228.
doi: 10.1016/j.watres.2011.07.026 pmid: 21864879[10] 赵丽红, 聂飞 . 水处理高级氧化技术研究进展[J]. 科学技术与工程, 2019,19(10):1-9. ZHAO L H, NIE F . Research progress in advanced oxidation technology for water treatment[J]. Science Technology and Engineering, 2019,19(10):1-9.
[11] 余臻 . 光催化氧化技术在水处理中的应用及研究进展[J]. 绿色科技, 2019(8):62-63. [12] 周明毅, 魏琛, 盛贵尚 , 等. 紫外活化过硫酸钠降解水中三唑酮的效能[J]. 环境工程学报, 2019,13(4):810-817. ZHOU M Y, WEI C, SHENG G S , et al. Degradation of triadimefon in water by UV irradiation-activated sodium persulfate process[J]. Chinese Journal of Environmental Engineering, 2019,13(4):810-817.
[13] BARAKAT M A, TSENG J M, HUANG C P . Hydrogen peroxide-assisted photocatalytic oxidation of phenolic compounds[J]. Applied Catalysis B:Environmental, 2005,59(1):99-104.
[14] CRITTENDEN J C, HU S M, HAND D W , et al. A kinetic model for H2O2/UV process in a completely mixed batch reactor[J]. Water Research, 1999,33(10):2315-2328.
doi: 10.1080/03601234.2019.1571365 pmid: 30729853[15] 朱欢欢, 孙韶华, 冯桂学 , 等. 紫外联用高级氧化技术处理饮用水应用进展[J]. 水处理技术, 2019,45(3):1-7. [16] DING W, BOLTON J R, HOFMANN R . Medium pressure UV combined with chlorine advanced oxidation for trichloroethylene destruction in a model water[J]. Water Research, 2012,46(15):4677-4686.
doi: 10.1016/j.watres.2012.06.007[17] XIANG Y Y, FANG J Y, SHANG C . Kinetics and pathways of ibuprofen degradation by the UV/chlorine advanced oxidation process[J]. Water Research, 2016,90:301-308.
doi: 10.1016/j.watres.2015.11.069 pmid: 26748208[18] SICHEL C, GARCIA C, ANDRE K . Feasibility studies:UV/chlorine advanced oxidation treatment for the removal of emergin contaminants[J]. Water Research, 2011,45(19):6371-6380.
doi: 10.1016/j.watres.2011.09.025 pmid: 22000058[19] 王中兰, 陈菊, 冯碧敏 . 高效液相色谱法测定诺氟沙星滴眼液中诺氟沙星含量[J]. 哈尔滨医药, 2006,26(1):10-11. [20] WATTS M J, LINDEN K G . Chlorine photolysis and subsequent OH radical production during UV treatment of chlorinated water[J]. Water Research, 2007,41(13):2871-2878.
doi: 10.1016/j.watres.2007.03.032 pmid: 17498769[21] 伊学农, 方佳男, 高玉琼 , 等. 紫外线-氯联合高级氧化体系降解水中的萘普生[J]. 环境工程学报, 2019,13(5):1030-1037. YI X N, FANG J N, GAO Y Q , et al. Degradation of naproxen in water by UV/chlorine advanced oxidation process[J]. Chinese Journal of Environmental Engineering, 2019,13(5):1030-1037.
[22] NETA P, HUIE R E, ROSS A B . Rate constants for reactions of inorganic radicals in aqueous solution[J]. Journal of Physical and Chemical Reference Data, 1988,17(3):1027-1284.
[23] GUO K H, WU Z H, YAN S W , et al. Comparison of the UV/chlorine and UV/H2O2 processes in the degradation of PPCPs in simulated drinking water and wastewater:kinetics,radical mechanism and energy requirements[J]. Water Research, 2018,147:184-194.
doi: 10.1016/j.watres.2018.08.048 pmid: 30312791[24] WANG W L, WU Q Y, HUANG N , et al. Synergistic effect between UV and chlorine(UV/chlorine)on the degradation of carbamazepine:influence factors and radical species[J]. Water Research, 2016,98:190-198.
doi: 10.1016/j.watres.2016.04.015 pmid: 27105033[25] 李国亭, 宋海燕, 刘秉涛 , 等. 光催化过程中羟基自由基的产生与效能[J]. 环境工程学报, 2012,6(10):3388-3392. LI G T, SONG H Y, LIU B T , et al. Production and contribution of hydroxyl radicals in photocatalytic oxidation process[J]. Chinese Journal of Environmental Engineering, 2012,6(10):3388-3392.
[26] 喻杰, 叶志伟, 党文悦 , 等. 紫外波长对UV/Cl2高级氧化去除水中有机物的影响[J]. 环境工程学报, 2019,13(3):577-585. YU J, YE Z W, DANG W Y , et al. Effect of ultraviolet wavelength on organic matter removal from water by UV/Cl2 advanced oxidation[J]. Chinese Journal of Environmental Engineering, 2019,13(3):577-585.
[27] YANG Y, CAO Y, JIANG J , et al. Comparative study on degradation of propranolol and formation of oxidation products by UV/H2O2 and UV/persulfate(PDS)[J]. Water Research, 2019,149:543-552.
doi: 10.1016/j.watres.2018.08.074 pmid: 30502740[28] WANG A Q, LIN Y L, XU B , et al. Kinetics and modeling otiodoform degradation during UV/chlorine advanced oxidation process[J]. Chemical Engineering Journal, 2017,323:312-319.
doi: 10.1016/j.watres.2016.08.011 pmid: 27544349[29] JAYSON G, PARSONS B, SWALLOW A J . Some simple,highly reactive,inorganic chlorinederivatives in aqueous solution:their formation using pulses of radiation and their role in the mechanism of the Fricke dosimeter[J]. Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, 1973,69:1597-1607.
[30] YUAN R X, WANG Z H, HU Y , et al. Probing the radical chemistry in UV/persulfate-based saline wastewater treatment:kinetics modeling and byproducts ide.pngication[J]. Chemosphere, 2014,109:106-112.
doi: 10.1016/j.chemosphere.2014.03.007 pmid: 24873714[31] DENG J, SHAO Y S, GAO N Y , et al. Degradation of the antiepileptic drug carbamazepine upon different UV-based advanced oxidation processes in water[J]. Chemical Engineering Journal, 2013,222:150-158.
doi: 10.1016/j.cej.2013.02.045[32] YANG Y, JIANG J, LU XL , et al. Production of sulfate radical and hydroxyl radical by reaction of ozone with peroxymonosulfate:a novel advanced oxidation process[J]. Environmental Science & Technology, 2015,49(12):7300-7339.
doi: 10.1021/es506362e pmid: 25988821[33] FANG J Y, FU Y, SHANG C . The roles of reactive species in micropollutant degradation in the UV/free chlorine system[J]. Environmental Science & Technology, 2014,48(3):1859-1868.
doi: 10.1021/es4036094 pmid: 24400681[34] BUXTON G V, GREENSTOCK C L, HELMAN WP , et al. Critical review of rate constants for reactions of hydrated electrons,hydrogen atoms and hydroxyl radicals (·OH/·O-) in aqueous solution [J]. Journal of Physical and Chemical Reference Data, 1988,17(2):513-886.
[35] WU Z, GUO K, FANG J , et al. Factors affecting the roles of reactive species in the degradation of micropollutants by the UV/chlorine process[J]. Water Research, 2017,126:351-360.
doi: 10.1016/j.watres.2017.09.028 pmid: 28985600 -
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